Zelda II: The Adventure of Link will keep you entertained for quite a while, although its quite difficult and... just beause its fun Kirby's Adventure woooo.
These are both the first two game I got for the VC and I thourght they were great purchases.

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Heres mine (all info is on the Wiki)
Dragons curse (one of the best games ever)(see wonderboy 3 : the dragons trap)
Comix zone (not to every ones tastes)
Mario kart 64
Gunstar heros (everyone must play this its in most gamers top tens)
Bomberman (multi only)
Streets of rage (good but two is better)
Zelda oot (0V0)
Punch out (good boxing game)
Gain ground (think gaunlet but way better)
Zelda (no intro)